Hygroscopic growth and cloud condensation nuclei activation are key processes for accurately modeling the climate impacts of organic particulate matter. Nevertheless, the microphysical mechanisms of these processes remain unresolved. Here we report complex thermodynamic behaviors, including humidity-dependent hygroscopicity, diameter-dependent cloud condensation nuclei activity, and liquid–liquid phase separation in the laboratory for biogenically derived secondary organic material representative of similar atmospheric organic particulate matter. These behaviors can be explained by the non-ideal mixing of water with hydrophobic and hydrophilic organic components. The non-ideality-driven liquid–liquid phase separation further enhances water uptake and induces lowered surface tension at high relative humidity, which result in a lower barrier to cloud condensation nuclei activation. By comparison, secondary organic material representing anthropogenic sources does not exhibit complex thermodynamic behavior. The combined results highlight the importance of detailed thermodynamic representations of the hygroscopicity and cloud condensation nuclei activity in models of the Earth’s climate system.
Ball milling was used to prepare two ultrafine magnetic biochar/Fe3O4 and activated carbon (AC)/Fe3O4 hybrid materials targeted for use in pharmaceutical removal by adsorption and mechanochemical degradation of pharmaceutical compounds. Both hybrid adsorbents prepared after 2 hours milling exhibited high removal of carbamazepine (CBZ), and were easily separated magnetically. These adsorbents exhibited fast adsorption of CBZ and tetracycline (TC) in the initial 1 hour. The biochar/Fe3O4 had a maximum adsorption capacity of 62.7 mg/g for CBZ and 94.2 mg/g for TC, while values obtained for AC/Fe3O4 were 135.1 mg/g for CBZ and 45.3 mg/g for TC respectively when data were fitted using the Langmuir expression. Solution pH values slightly affected the sorption of TC on the adsorbents, while CBZ sorption was almost pH-independent. The spent adsorbents with adsorbed CBZ and TC were milled to degrade the adsorbed pollutants. The adsorbed TC itself was over 97% degraded after 3 hours of milling, while about half of adsorbed CBZ were remained. The addition of quartz sand was found to improve the mechanochemical degradation of CBZ on biochar/Fe3O4, and its degradation percent was up to 98.4% at the dose of 0.3 g quarts sand/g adsorbent. This research provided an easy method to prepare ultrafine magnetic adsorbents for the effective removal of typical pharmaceuticals from water or wastewater and degrade them using ball milling.
Local atmospheric recirculation flows (i.e., river winds) induced by thermal contrast between wide Amazon rivers and adjacent forests could affect pollutant dispersion, but observational platforms for investigating this possibility have been lacking. Here we collected daytime vertical profiles of meteorological variables and chemical concentrations up to 500 m with a copter-type unmanned aerial vehicle during the 2019 dry season. Cluster analysis showed that a river-forest recirculation flow occurred for 23% (13 of 56) of the profiles. In fair weather, the thermally driven river winds fully developed for synoptic wind speeds below 4 m s−1, and during these periods the vertical profiles of carbon monoxide and total oxidants (defined as ozone and nitrogen dioxide) were altered. Numerical modeling shows that the river winds can recirculate pollution back toward the riverbank. There are implications regarding air quality for the many human settlements along the rivers throughout northern Brazil.
A simple and convenient method was used to prepare novel granular carbon nanotubes (CNTs) for enhanced adsorption of pharmaceuticals. By heating CNTs powder at 450 in air, followed by filtration, the obtained granular adsorbent exhibited high surface area and pore volume since the heating process produced some oxygen-containing functional groups on CNT surface, making CNTs more dispersible in the formation of granular cake. The porous granular CNTs not only had more available surfaces for adsorption but also were more easily separated from solution than pristine CNTs (p-CNTs) powder. This adsorbent exhibited relatively fast adsorption for carbamazepine (CBZ), tetracycline (TC) and diclofenac sodium (DS), and the maximum adsorption capacity on the granular CNTs was 369.5 mol/g for CBZ, 284.2 mol/g for TC and 203.1 mol/g for DS according to the Langmuir fitting, increasing by 42.4%, 37.8% and 38.0% in comparison with the pristine CNTs powder. Moreover, the spent granular CNTs were successfully regenerated at 400 in air without decreasing the adsorption capacity in five regeneration cycles. The adsorbed CBZ and DS were completely degraded, while the adsorbed TC was partially oxidized and the residual was favorable for the subsequent adsorption. This research develops an easy method to prepare and regenerate granular CNT adsorbent for the enhanced removal of organic pollutants from water or wastewater.
Nighttime vertical profiles of ozone, PM2.5 and PM10 particulate matter, carbon monoxide, temperature, and humidity were collected by a copter-type unmanned aerial vehicle (UAV) over the city of Manaus, Brazil, in central Amazon during the dry season of 2018. The vertical profiles were analyzed to understand the structure of the urban nighttime boundary layer (NBL) and pollution within it. The ozone concentration, temperature, and humidity had an inflection between 225 and 350 m on most nights, representing the top of the urban NBL. The profile of carbon monoxide concentration correlated well with the local evening vehicular congestion of a modern transportation fleet, providing insight into the surface-atmosphere dynamics. In contrast, events of elevated PM2.5 and PM10 concentrations were not explained well by local urban emissions, but rather by back trajectories that intersected regional biomass burning. These results highlight the potential of the emerging technologies of sensor payloads on UAVs to provide new constraints and insights for understanding the pollution dynamics in nighttime boundary layers in urban regions.
Volatile organic compounds (VOCs) emitted from forests are important chemical components that affect ecosystem functioning, atmospheric chemistry, and regional climate. Temperature differences between a forest and an adjacent river can induce winds that influence VOC fate and transport. Quantitative observations and scientific understanding, however, remain lacking. Herein, daytime VOC datasets were collected from the surface up to 500 m over the "Rio Negro" river in Amazonia. During time periods of river winds, isoprene, α-pinene, and β-pinene concentrations increased by 50, 60, and 80% over the river, respectively. The concentrations at 500 m were up to 80% greater compared to those at 100 m because of the transport path of river winds. By comparison, the concentration of methacrolein, a VOC oxidation product, did not depend on river winds or height. The differing observations for primary emissions and oxidation products can be explained by the coupling of timescales among emission, reaction, and transport. This behavior was captured in large-eddy simulations with a coupled chemistry model. The observed and simulated roles of river winds in VOC fate and transport highlight the need for improved representation of these processes in regional models of air quality and chemistry−climate coupling.
<p>Local atmospheric circulation induced by wide rivers in Amazonia can strongly affect the transport of urban, industrial, fire, and forest emissions. Herein, a copter-type unmanned aerial vehicle (UAV) operated from a boat was used to collect vertical profiles of meteorological parameters and chemical concentrations during Sep-Oct 2019 of the dry season. Sensor packages mounted on the UAV measured wind speed and direction together with concentrations of carbon monoxide (CO) and total oxidants (O<sub>x</sub>, defined as O<sub>3</sub> + NO<sub>2</sub>). Multivariate statistical analysis identified distinguishing patterns for meteorological variables. The occurrence of river breeze circulations was linked to meteorological conditions from in-situ measurement and satellite images. Vertical profiles of chemical concentrations both from in-situ measurements and large eddy simulations confirmed that under some conditions a river breeze can facilitate pollutant mixing perpendicular to the river orientation. The results of this study advance an urgent need to quantify the occurrence and the properties of river breeze circulations in respect to microscale chemical dispersion, air quality, and human health.</p>
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